Homogeneous nucleation rates of supercooled water measured in single levitated microdroplets

Krämer, Benedikt; Hübner, Oskar; Vortisch, H.; Wöste, L.; Leisner, Thomas; Schwell, Martin; Rühl, E.; Baumgärtel, H.

doi:10.1063/1.479946

Cited by 176 publications

(215 citation statements)

References 45 publications

(47 reference statements)

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“…4͒. The optical arrangement is similar to that reported by Krämer et al 10 A collimating lens fastened directly to the chamber in place of a window minimizes Fabry-Pérot interference that would result from passing the spherical wave front through the two parallel flat surfaces of a window. A second lens focuses the scattered light through an aperture ͑approximately 1.5 mm͒ to filter off-axis radiation and a third lens recollimates the light onto the CCD detector of a video camera.…”

Section: Collection Of Angular Light Scatteringsupporting

confidence: 54%

“…13 When, for example, Krämer et al 10 systematically varied the temperature, the measured ice crystal nucleation rate increased by a factor of 70 as the temperature was reduced by just 1 K. Precise control of the thermodynamic state is thus critical to the measurement of nucleation rates. Only able to regulate the relative humidity ͑RH͒ within ±0.5% RH during repeated experiments, Hamza et al 9 reported nucleation rates that varied by a factor of 300.…”

Section: Introductionmentioning

confidence: 99%

“…From repeated measurements of this incubation time in levitated droplets under similar conditions, a number of authors have inferred nucleation rates. Krämer et al 10 measured the nucleation rate of ice crystals in supercooled water by repeatedly injecting and trapping warm droplets into a cold balance; in a similar experiment Weidinger et al 12 measured homogeneous and heterogeneous crystal nucleation rates from n-alkane melts. Both studies detected crystallization through changes in optical properties.…”

Section: Introductionmentioning

confidence: 99%

“…1 Electrostatic levitation has therefore found many applications in aerosol and materials research, including investigations of aqueous solution thermodynamics and crystal nucleation kinetics. [1][2][3][4][5][6][7][8][9][10][11][12] Several researchers have recently employed electrostatic levitation to quantitatively investigate crystal nucleation kinetics in a variety of chemical systems. Nucleation is a stochastic process; when a supersaturated or supercooled state is created, nucleation occurs after a delay or incubation time.…”

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Single-particle levitation system for automated study of homogeneous solute nucleation

Olsen

Flagan

Kornfield

2006

Review of Scientific Instruments

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We present an instrument that addresses two critical requirements for quantitative measurements of the homogeneous crystal nucleation rate in supersaturated aqueous solution. First, the need to perform repeated measurements of nucleation incubation times is met by automating experiments to enable programmable cycling of thermodynamic conditions. Second, the need for precise and robust control of the chemical potential in supersaturated aqueous solution is met by implementing a novel technique for regulating relative humidity. The apparatus levitates and weighs micron-sized samples in an electric field, providing access to highly supersaturated states. We report repeated observations of the crystal nucleation incubation time in a supersaturated aqueous sodium chloride droplet, from which we infer the nucleation rate.

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Section: Collection Of Angular Light Scatteringsupporting

confidence: 54%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Single-particle levitation system for automated study of homogeneous solute nucleation

Olsen

Flagan

Kornfield

2006

Review of Scientific Instruments

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show abstract

“…1,56 In this study, we have selected a subset [56][57][58][59][60][61][62][63][64][65][66][67][68] of the available data sets for the purposes of constraining the new parameterization. The criteria for selection were (i) minimal and well defined uncertainties, (ii) good reproducibility within the data set, and (iii) an internal droplet pressure of about 1 bar.…”

Section: Fitting the Cnt-based Model To Experimental Datamentioning

confidence: 99%

A physically constrained classical description of the homogeneous nucleation of ice in water

Koop

Murray

2016

The Journal of Chemical Physics

117

155

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Liquid water can persist in a supercooled state to below 238 K in the Earth's atmosphere, a temperature range where homogeneous nucleation becomes increasingly probable. However, the rate of homogeneous ice nucleation in supercooled water is poorly constrained, in part, because supercooled water eludes experimental scrutiny in the region of the homogeneous nucleation regime where it can exist only fleetingly. Here we present a new parameterization of the rate of homogeneous ice nucleation based on classical nucleation theory. In our approach, we constrain the key terms in classical theory, i.e., the diffusion activation energy and the ice-liquid interfacial energy, with physically consistent parameterizations of the pertinent quantities. The diffusion activation energy is related to the translational self-diffusion coefficient of water for which we assess a range of descriptions and conclude that the most physically consistent fit is provided by a power law. The other key term is the interfacial energy between the ice embryo and supercooled water whose temperature dependence we constrain using the Turnbull correlation, which relates the interfacial energy to the difference in enthalpy between the solid and liquid phases. The only adjustable parameter in our model is the absolute value of the interfacial energy at one reference temperature. That value is determined by fitting this classical model to a selection of laboratory homogeneous ice nucleation data sets between 233.6 K and 238.5 K. On extrapolation to temperatures below 233 K, into a range not accessible to standard techniques, we predict that the homogeneous nucleation rate peaks between about 227 and 231 K at a maximum nucleation rate many orders of magnitude lower than previous parameterizations suggest. This extrapolation to temperatures below 233 K is consistent with the most recent measurement of the ice nucleation rate in micrometer-sized droplets at temperatures of 227-232 K on very short time scales using an X-ray laser technique. In summary, we present a new physically constrained parameterization for homogeneous ice nucleation which is consistent with the latest literature nucleation data and our physical understanding of the properties of supercooled water. C 2016 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license

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Sensitivity of liquid clouds to homogenous freezing parameterizations

Herbert

Murray

Dobbie

et al. 2015

Geophysical Research Letters

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Water droplets in some clouds can supercool to temperatures where homogeneous ice nucleation becomes the dominant freezing mechanism. In many cloud resolving and mesoscale models, it is assumed that homogeneous ice nucleation in water droplets only occurs below some threshold temperature typically set at −40°C. However, laboratory measurements show that there is a finite rate of nucleation at warmer temperatures. In this study we use a parcel model with detailed microphysics to show that cloud properties can be sensitive to homogeneous ice nucleation as warm as −30°C. Thus, homogeneous ice nucleation may be more important for cloud development, precipitation rates, and key cloud radiative parameters than is often assumed. Furthermore, we show that cloud development is particularly sensitive to the temperature dependence of the nucleation rate. In order to better constrain the parameterization of homogeneous ice nucleation laboratory measurements are needed at both high (>−35°C) and low (<−38°C) temperatures.Key PointsHomogeneous freezing may be significant as warm as −30°CHomogeneous freezing should not be represented by a threshold approximationThere is a need for an improved parameterization of homogeneous ice nucleation

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Homogeneous nucleation rates of supercooled water measured in single levitated microdroplets

Cited by 176 publications

References 45 publications

Single-particle levitation system for automated study of homogeneous solute nucleation

Single-particle levitation system for automated study of homogeneous solute nucleation

A physically constrained classical description of the homogeneous nucleation of ice in water

Sensitivity of liquid clouds to homogenous freezing parameterizations

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